题目: | quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
作者: | shuang liu1#, zhiyi wu1#, zhijie zhu1#, kai feng1, yuxuan zhou1, xinge hu1, xiong huang2, binbin zhang3, xudong dong1, yueru ma1, kaiqi nie4, jiahui shen1, zidi wang1, jiari he5, jiaqi wang1, yu ji1, binhang yan4, qingfeng zhang3, alexander genest6, xiaohong zhang1, chaoran li1, 7*, bo wu2, xingda an1*, günther rupprechter6 & le he1* |
单位: | 1institute of functional nano & soft materials (funsom) and jiangsu key laboratory of advanced negative carbon technologies, soochow university, suzhou, 215123, pr china. 2guangdong provincial key laboratory of optical information materials and technology, institute of electronic paper displays, south china academy of advanced optoelectronics, south china normal university, guangzhou 510006, pr china. 3college of chemistry and molecular sciences, wuhan university, wuhan, hubei, 430072, pr china. 4department of chemical engineering, tsinghua university, beijing 100084, china 5state key laboratory of crystal materials, institute of crystal materials, shandong university, jinan, shandong, 250100, pr china. 6institute of materials chemistry, tu wien, wien 1060, austria. 7jiangsu key laboratory for carbon-based functional materials & devices, soochow university, suzhou, 215123, jiangsu, pr china. |
摘要: | plasmonic photocatalysis enabled by the unique localized surface plasmon resonance represents a promising approach for efficient solar energy conversion. elucidating the distinct plasmonic catalytic mechanisms and quantification of their effect is crucial yet highly challenging, due to their complex and synergistic nature. herein, we achieve the differentiation and quantification of thermal as well as various non-thermal reaction mechanisms in prototypical au-[fe(bpy)3]2 antenna-reactor photocatalysts using water splitting as test reaction. through modification of the resonance condition and connection schemes, non-thermal plasmonic charge and energy transfer mechanisms are selectively shielded. it is found that plasmonic charge carrier-induced photochemistry dominates the photocurrent (~57%) in a reducing, hydrogen evolution environment; whereas resonant plasmonic energy transfer dominates (~54%) in an oxidative, oxygen evolution environment. our approach provides generalized and fundamental understandings on the role of surface plasmons in photocatalysis as well as important design principles for plasmonic photocatalysts towards distinct reaction types and catalyst configurations. |
影响因子: | 14.7 |
分区情况: | 一区 |
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责任编辑:郭佳